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化学进展 2021, Vol. 33 Issue (8): 1311-1322 DOI: 10.7536/PC200750 前一篇   后一篇

• 综述 •

多相催化过硫酸盐工艺处理水环境中有机污染物的非自由基过程

刘佳, 史俊, 付坤, 丁超, 龚思成, 邓慧萍*()   

  1. 同济大学 长江水环境教育部重点实验室 上海污染控制与生态安全研究院 环境科学与工程学院 上海 200092
  • 收稿日期:2020-07-22 修回日期:2020-11-10 出版日期:2021-08-20 发布日期:2020-12-28
  • 通讯作者: 邓慧萍
  • 基金资助:
    国家水体污染控制与治理科技重大专项(2017ZX07201003-02)
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Heterogeneous Catalytic Persulfate Oxidation of Organic Pollutants in the Aquatic Environment: Nonradical Mechanism

Jia Liu, Jun Shi, Kun Fu, Chao Ding, Sicheng Gong, Huiping Deng()   

  1. Key Laboratory of Yangtze River Water Environment, Ministry of Education, Shanghai Institute of Pollution Control and Ecological Security, College of Environmental Science and Engineering, Tongji University,Shanghai 200092, China
  • Received:2020-07-22 Revised:2020-11-10 Online:2021-08-20 Published:2020-12-28
  • Contact: Huiping Deng
  • Supported by:
    Major Science and Technology Program for Water Pollution Control and Treatment of China(2017ZX07201003-02)

20世纪80年代至今,水处理技术中的高级氧化过程(AOP)已被广泛研究及应用。然而水体中的有机污染物仍因种类繁多和降解难易不同困扰着研究者们,因此对于AOP的机理过程需要更深入的分析认识,以利于技术的进一步发展及应用。AOP中的过硫酸盐氧化工艺近年来得到大量关注,其自由基机理的关键活性物种是·OH 和·SO4-。非自由基机理分为1O2氧化和PS直接氧化(也称电子转移),某些体系中高价态金属也直接或间接地参与氧化过程。但非自由基过程的发生机理及优势特点仍存在争议。本文综述了基于多相催化过硫酸盐高级氧化过程处理水中有机污染物的最新研究,阐述反应机理及其分析手段,并指出当前研究可能存在的问题。对于过硫酸盐高级氧化工艺中非自由基过程的未来研究方向及应用前景提出展望。

关键词： 高级氧化过程, 过硫酸盐, 非自由基机理, 单线态氧, 电子转移

Since the 1980s, the advanced oxidation process(AOP) in water treatment technology has been widely researched and applied. However, organic pollutants in water still plague scholars due to their wide variety and difficulty in degradation. Therefore, the mechanism of AOP needs to be clearly understood and get deeper into, which is conducive to technological application. As a typical AOP, the peroxymonosulfate & peroxydisulfate oxidation process has received a lot of attention in recent years, whereas there are still numerous disputes on the mechanism, lacking a unified understanding. The key reactive species of free radical process are generally ·OH and ·SO4-. Nonradical process contains 1O2 oxidation and peroxymonosulfate & peroxydisulfate oxidation(known as an electron transfer process), and high valence metal also participates in the oxidation process directly or indirectly. The specific mechanism of nonradical processes are still controversial, also the advantages and disadvantages. For the above reasons, this paper reviews the latest researches on the treatment of organic pollutants based on heterogeneous catalytic persulfate oxidation process in water, explains the reaction mechanism and the analysis methods, and points out the possible current research problems. Prospects for the future research direction and the application perspective of persulfate oxidation are proposed, with an emphasis on nonradical processes.

Contents

1 Introduction

2 Mechanism of singlet oxygen

2.1 Activated by ketone group

2.2 Produced by superoxide anion radical

2.3 Produced by PMS anion radical

2.4 Other ways for producing singlet oxygen

3 Mechanism of electron transfer

3.1 Catalyst-mediated electron transfer

3.2 Activated persulfate on the surface of catalyst

4 Mechanism of high valence metal

5 Analysis methods and catalyst deactivation

5.1 Analysis methods

5.2 Catalyst deactivation

6 Conclusion and outlook

Key words: advanced oxidation process, persulfate, nonradical mechanism, singlet oxygen, electron transfer
()
图1 2015年至2020年Web of Science过硫酸盐氧化工艺去除有机物染物及基于非自由基机理的发表物数量
Fig. 1 Number of publications on persulfate oxidation process for organic pollutants removal and nonradical mechanism on Web of Science during 2015 to 2020
表1 多相催化过硫酸盐氧化工艺研究成果
Table 1 Researches on heterogeneous catalytic persulfate oxidation process
Pollutant, Concentration Catalyst, Dosage
(*0.1 g/L)		 Oxidant, Dosage Degradation(%)/
Adsorption(%)		 Mechanism/nonradical process proportion pH/
Reaction time(min)		 Cycles/
ΔDegradation(%)		 ref
Phenol, 20 ppm N-SWCNT, 1 PMS, 6.5 mM 100/- Electron transfer/key role Neutral/30 3/11 23
Sulfamethoxazole, 20 μM FeCo2S4-C3N4, 0.1 PMS, 0.15 mM 92/15 1O2/dominated 6.5/15 3/24 24
Phenol, 100 μM MnO2, 4 PDS, 4 mM 100/12 1O2/100% 6.5/180 -/- 25
Tetracycline, 35 mg/L NMC, 1 PDS, 1 mM 100/23.7 Electron transfer/key role 7/120 5/21 26
Oxytetracycline, 250 mg/L Fe/C, 5 PMS, 1 mM 100/- 1O2/partial 8.2/30 -/- 27
4-Chlorophenol, 0.1 mM Ni-NiO, 2 PDS, 0.2 mM 80/- Electron transfer/partial 7/60 3/5 28
Atrazine, 10 mg/L Titanomagnetite, 80 PDS, 5.0 mM 92/- FeⅣ/partial 6.3/90 5/35 29
Bisphenol A, 0.09 mM Cu-rGO LDH, 2.5 PMS, 3 mM 99/- 1O2/100% Neutral/40 3/10 30
Oxytetracycline, 40 μM Co3O4-MC, 2 PMS, 0.5 mM 95/17 1O2/partial 5/12 5/4 31
2,4-Dichlorophenol, 50 μM CuFe oxide, 2 PDS, 0.2 mM 100/limited Electron transfer/100% 5.8/120 3/15 32
Sulfamethoxazole, 5 mg/L Fe3C@NCNTs, 1 PDS, 1 mM 98/48 1O2/primary Neutral/100 4/80 33
Bisphenol A, 0.1 mM NCN, 1 PMS, 2 mM 100/25 1O2/primary 6.7/2 5/0 14
Phenol, 20 mg/L PPy-T, 1 PMS, 3.25 mM 97/- Electron transfer/dominated 2.8/120 3/20 34
4-Chlorophenol, 40 ppm CuOMgO/Fe3O4, 2 PMS, 2 mM 100/10 1O2/100% Neutral/40 -/- 35
2,4-Dichlorophenol, 5 μM CuO, 2 PDS, 40 μM 100/limited Electron transfer/100% 5.8/60 -/- 17
Trichlorophenol, 0.1 mM Au/Al2O3, 2.5 PMS, 1 mM 100/limited Electron transfer/dominated 7/60 -/- 36
2,4-Dichlorophenol, 0.05 mM CNT, 1 PDS, 0.05 mM 100/25 1O2, Electron transfer/100% 6.5/30 5/50 37
2,4-Dichlorophenol, 0.03 mM Fe/S-CNTs, 1 PDS, 0.03 mM 95/40 Electron transfer/key role 7/30 4/31 38
p-Chloroaniline, 0.5 mM CuO, 5 PDS, 2.3 mM 71.5/5 Electron transfer/key role 7/350 -/- 39
2,4,6-Trichlorophenol,0.1 mM CuO/rGO, 1 PDS, 2.5 mM 80/limited Electron transfer/key role 6/180 -/- 40
Bisphenol A, 5 mg/L CuO, 1 PMS, 0.5 mM 100/5 1O2/dominated 7.2/60 5/5 41
Diclofenac, 0.01 g/L CNOMS, 1 PMS, 0.2 g/L 98/- 1O2/partial 8.3/20 4/15 42
Ciprofloxacin, 0.03 mM CuO, 5 PDS, 1 mM 100/41 Electron transfer/dominated 8/60 5/0 43
Acid Red 1, 50 μM CuO-CF, 20 PMS, 0.5 mM 100/limited 1O2/dominated 10/10 5/limited 44
Sulfonamides, 40 μM rGO, 1 PDS, 0.6 mM 100/- 1O2/100% 5/30 -/- 45
图2 碳纳米管催化过二硫酸盐产生单线态氧的过程[50]
Fig. 2 Generation of1O2 by PDS catalyzed by CNTs[50]
图3 苯醌催化过一硫酸盐产生单线态氧的过程[47]
Fig. 3 Generation of1O2 by PMS catalyzed by BQ[47]
图4 二氧化锰催化过二硫酸盐产生单线态氧的过程[24]
Fig. 4 Generation of1O2 by PDS catalyzed by MnO2[24]
图5 产生单线态氧的几种方式
Fig. 5 Several ways for producing singlet oxygen
图6 过硫酸盐与碳纳米管形成活性复合物[48]
Fig. 6 Reactive Complexes formed by PS and CNTs[48]
图7 取代基对5种磺胺类药物降解机理的影响[44]
Fig. 7 Effects of substituents on degradation mechanism of five sulfonamides[44]
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